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標題: | 由大至小調整超薄奈米催化劑尺寸訂製載子傳輸 Tailoring Carrier Transport Through Top-Down Structural Manipulation of Ultrathin Nanocatalysts |
作者: | 桀 亞 Jeyavelan Muthu |
指導教授: | 謝馬利歐 Mario Hofmann |
關鍵字: | 2D-TMDs,梯度,HER,熱電子,CO2RR, 2D-TMDs,Gradient,HER,Hot electron,CO2RR, |
出版年 : | 2023 |
學位: | 博士 |
摘要: | 在全球暖化和急需解決環境永續性問題的背景下,可穩續生產化學製品顯得尤為緊迫。傳統的製造過程往往仰賴高耗能的方法並伴隨大量的溫室氣體排放,造成顯著的氣候變化。因此,找到創新和穩定的製造過程的需求變得十分迫切。奈米技術已經在催化劑的改進以及新現象上有顯現出巨大的潛力。
然而,複雜的奈米結構限制了開發的量能。本論文探討了由上而下結構調控的超薄催化劑,重點聚焦在不同奈米尺度約束下的催化性能。 首先,實現了隨空間變化形態的二維過度金屬二硫化物(2D-TMDs),並對不同型態之電催化性能進行了研究。研究顯示,在2D-TMDs的內部均質電荷傳遞受到了限制,這在產氫反應(HER)中有著顯著的變化。對圍觀梯度的MoS2和WS2器件的電化學特性的統計研究指出了未補償電阻對於過電位和Tafel斜率的主導效應。本研究引入了HER極化校正方法發現了先前作業上對HER機制的潛在錯誤,並強調了在不同形態下載體傳輸對2D-TMDs電化學性質的影響。 其次,我們實現了空間上大小分布公分尺度的等離子過度金屬(PTM)奈米結構。透過採用超薄金(Au)梯度奈米結構,混合交互作用達到性能的提升。研究顯示出內部形成了一個強健的電場,該電場有效的與等離子的自由度耦合,產生縱向的等離子高峰。這種創新的方式促使光能高效解離,通过光催化轉化得到了卓越的CO產物選擇性,展示了梯度等離子體结夠在推動綠色能源轉換和儲存方面實際應用的潜力。 對結構調控、電荷傳遞動力學和等離子交互作用的全面探索為先進材料的發展開闢了道路,對永續能源技術具有重要的影響。 In light of global warming and the imperative need to address environmental sustainability, the sustainable production of chemicals is of utmost urgency. Traditional chemical manufacturing processes often rely on energy-intensive methods and generate substantial greenhouse gas emissions, contributing significantly to climate change. Consequently, there is a critical demand for innovative and sustainable approaches to chemical production Nanotechnology has shown great promise to achieve this goal in the form of improved catalysis and novel phenomena. However, the complex formation of nanostructures has limited the throughput of discovery. This thesis explores top-down structural manipulation of ultrathin catalysts, focusing on their catalytic performance under varying nanoscopic confinement. First, 2D transition metal dichalcogenides (2D-TMDs) with a spatially varying morphologies were achieved and their morphological impact on the electrocatalytic performance was investigated. The study demonstrated that limitations in homogeneous charge transfer within 2D-TMDs significantly contribute to variations in hydrogen evolution reactions (HER). Statistical electrochemical characterization of microscopic gradient MoS2 and WS2 devices reveals the dominating effect of uncompensated resistance on overpotential and Tafel slope. The study introduces a HER polarization correction approach, uncovering potential errors in previous assignments of the HER mechanism and emphasizing the impact of morphology-dependent carrier transport on the electrochemical properties of 2D-TMDs. Second, we achieved a centimeter scale plasmonic transition metal (PTM) nanostructures with spatially varying size distribution. Through the implementation of an ultrathin gold (Au) gradient nanostructure, hybrid interactions achieve enhanced performance. The study revealed the formation of a robust internal electric field that efficiently couples with the plasmonic degree of freedom, yielding longitudinal plasmonic peaks. This innovative approach facilitates efficient dissociation of hot carriers, demonstrated through photocatalytic conversion. Hot-electron-assisted CO2 reduction achieves a remarkable CO product with high selectivity, showcasing the potential of gradient plasmonic structures for advancing practical applications in green energy conversion and storage. The comprehensive exploration of structural manipulation, charge transfer kinetics, and plasmonic interactions opens avenues for the development of advanced nanomaterials with significant implications for sustainable energy technologies. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/91609 |
DOI: | 10.6342/NTU202400100 |
全文授權: | 同意授權(限校園內公開) |
顯示於系所單位: | 物理學系 |
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